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US5093361A - D-2-(6-methoxy-2-naphthyl)-propionic acid and pharmaceutical compositions containing it - Google Patents

D-2-(6-methoxy-2-naphthyl)-propionic acid and pharmaceutical compositions containing it Download PDF

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US5093361A
US5093361A US07/485,084 US48508490A US5093361A US 5093361 A US5093361 A US 5093361A US 48508490 A US48508490 A US 48508490A US 5093361 A US5093361 A US 5093361A
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nxtio
naphthyl
methoxy
pharmaceutical compositions
propionic acid
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Valentina Reiner
Caterina Sarda
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Farma Resa Srl
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C327/00Thiocarboxylic acids
    • C07C327/20Esters of monothiocarboxylic acids
    • C07C327/32Esters of monothiocarboxylic acids having sulfur atoms of esterified thiocarboxyl groups bound to carbon atoms of hydrocarbon radicals substituted by carboxyl groups
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K31/00Medicinal preparations containing organic active ingredients
    • A61K31/21Esters, e.g. nitroglycerine, selenocyanates
    • A61K31/265Esters, e.g. nitroglycerine, selenocyanates of carbonic, thiocarbonic, or thiocarboxylic acids, e.g. thioacetic acid, xanthogenic acid, trithiocarbonic acid

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  • the present invention relates to an optically active isomer of a derivative of d-2-(6-methoxy-2-naphthyl)-propionic acid, namely of the active principle known as Naproxen; the invention relates as well to pharmaceutical compositions containing the said derivative.
  • Naproxen is known since a number of years and is included among the substances having anti-inflammatory, analgesic and anti-pyretic activity. Its main therapeutic use is the treatment of rheumatoid arthritis and of other degenerative forms having phlogistic features.
  • alpha-mercaptopropionylglycine is a compound known as well, possessing also anti-inflammatory activity besides the mucolytic activity.
  • the diastereoisomer of the present invention to the prevailing anti-inflammatory activity which is characteristic both of Naproxen and more remarkably of the derivatives being the subject of the European Patent 124.925, adds a specific analgesic activity which is definitely higher than that the of the corresponding racemic compound.
  • the product of the reaction carried out between the acid chloride of d-2-(6-methoxy-2-naphthyl)-propionic acid and (2-mercapto-propionyl)-glycine in the presence of a base is poured in water, then an acidification is carried out with hydrochloric acid and the solid thus precipitated is filtered.
  • an acidification is carried out with hydrochloric acid and the solid thus precipitated is filtered.
  • repeated fractionated crystallizations, of the racemic one are carried out, using ethyl acetate as the crystallization solvent, until a product having constant melting point (180-1° C.) is obtained.
  • each rat received an injection of 0.1 ml of a 1% w/v suspension of carrageenan in sterile 0.9% saline, beneath the plantar aponeurosis of the left hind paw.
  • the volume of the paw was measured (in arbitrary units) before and 1.5, 3 and 6 hours after the irritant injection.
  • the results are reported in the table 2, from which it can be observed not only that both diastereoisomers administered by oral route induce a significant inhibition of the carrageenan induced oedema, but also that d-l isomer is slightly less active than the d-d isomer.
  • the measurement of the paw volume was carried out before the injection and at 0.5, 1 and 2.5 hours after the injection.
  • Groups of 10 rats (Wistar-Charles River) were dosed orally with either vehicle (0.5% tragacanth) or test compounds (d-d and d-1 Nxtio) at a costant volume of 10 ml/kg according to the treatment table 1.
  • each rat received an intraperitoneal injection of 1.0 ml of 1% solution of acetic acid. They were then placed in individual cages and the number of writhes elicited by each rat in the following 25 minute period was recorded.
  • Each rat received an injection of 0.1 ml of a 20% suspension of Brewer's yeast in distilled water beneath the plantar aponeurosis of the left hind paw.
  • the pain thresholds of the inflamed and normal hind paws were again measured at 1, 2 and 4 hours after dosing.
  • compositions according to the present invention comprise as the active ingredient the (d-d) diastereoisomer together with the standard vehicles and excipients.
  • the dosages of active principles shall be still those of the corresponding composition based on Naproxen whereby the therapeutical effect is obviously increased.

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  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
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  • Medicinal Chemistry (AREA)
  • Pharmacology & Pharmacy (AREA)
  • Emergency Medicine (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Animal Behavior & Ethology (AREA)
  • General Health & Medical Sciences (AREA)
  • Public Health (AREA)
  • Veterinary Medicine (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Acyclic And Carbocyclic Compounds In Medicinal Compositions (AREA)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)

Abstract

The S-[d-2-(6-methoxy-2-naphthyl)-propionyl]d-2-mercaptopropionamidoacetic acid having formula: ##STR1## has improved therapeutic properties not only in comparison with the starting active principle, namely Naproxen, but also with respect to the corresponding racemic derivative, namely the (d,l) compound.

Description

The present invention relates to an optically active isomer of a derivative of d-2-(6-methoxy-2-naphthyl)-propionic acid, namely of the active principle known as Naproxen; the invention relates as well to pharmaceutical compositions containing the said derivative.
Naproxen is known since a number of years and is included among the substances having anti-inflammatory, analgesic and anti-pyretic activity. Its main therapeutic use is the treatment of rheumatoid arthritis and of other degenerative forms having phlogistic features.
In turn, alpha-mercaptopropionylglycine is a compound known as well, possessing also anti-inflammatory activity besides the mucolytic activity.
The derivatives obtained by combining the said two active principles are the object of the European Patent No. 124.925, which thus claims compounds having the following general formula: ##STR2## wherein X is hydrogen or a radical selected from among organic radicals or inorganic radicals, non toxic and pharmaceutically acceptable bases, radicals of basic aminoacids and radicals of basic antibiotics.
The characteristics and properties of the above mentioned compounds in the racemic form, namely the (d,l) form, are given in the specification and in the examples of this European Patent.
It has been now found and is the object of the present invention that the (d,d) diastereoisomer of the compound directly obtained from Naproxen and alpha-mercaptopropionylglycine has surprisingly specific properties which are superior not only to respect with the starting active principle, namely Naproxen, but also with respect to the corresponding (d,l) racemic compound.
This greater activity over Naproxen is mainly seen in the lack of ulcerogenicity which is on the contrary the main drawback of Naproxen as regards the therapeutical use; whereas in comparison with the corresponding racemic compound, the diastereoisomer of the present invention has greater analgesic activity.
Otherwise stated, the diastereoisomer of the present invention to the prevailing anti-inflammatory activity which is characteristic both of Naproxen and more remarkably of the derivatives being the subject of the European Patent 124.925, adds a specific analgesic activity which is definitely higher than that the of the corresponding racemic compound.
It is evident that the therapeutical use of these substances makes the symptomatic activity, namely the analgesic one, of the utmost importance.
As regards the preparation of the diastereoisomer of the present invention, reference is made to the specification and examples of European Patent 124.925, particularly examples 1a and 1b of this patent, which is herein included by reference.
Thus according to the process studied with respect to the present invention, the product of the reaction carried out between the acid chloride of d-2-(6-methoxy-2-naphthyl)-propionic acid and (2-mercapto-propionyl)-glycine in the presence of a base is poured in water, then an acidification is carried out with hydrochloric acid and the solid thus precipitated is filtered. For the separation of the desired (d,d) form; repeated fractionated crystallizations, of the racemic one are carried out, using ethyl acetate as the crystallization solvent, until a product having constant melting point (180-1° C.) is obtained.
The obtained compound has been subjected to elemental analysis with the following results:
Calculated for C19 H21 NO5 S: %C 60.78; %H 5,63; %N 3,73; %S 8,54
Found: %C 61.02; %H 5.59; %N3,71; %S 8.63.
The (d,d) diastereoisomer of the invention is a crystalline solid having [alpha]D 20 +201.01 (C=1, methanol).
It is soluble in ethanol, methanol and acetone, a little soluble in hot ethyl acetate and insoluble in water.
By carrying out the TLC analysis with chloroform: glacial acetic acid: water (85:15:0.5) as the eluant system, a value Rf =0.75 is obtained whereas the (d,l) diastereoisomer has Rf =0.70.
The already mentioned properties of the diastereoisomer according to the invention have been confirmed by the pharmacological tests which are hereinafter shortly reported (the compound of the invention is indicated in abbreviated form has d-d Nxtio whereas the other diastereoisomer is abbreviated as d-1 Nxtio).
As regards the anti-inflammatory activity, the standard tests by means of carrageenan induced oedema and dextran induced oedema were performed whereas for the analgesic activity the writhing test and the Randall-Selitto test have been carried out.
1. Carrageenan induced oedema in the rat
Groups of 8 rats (Wistar-Charles River) have been orally administered with:
(i) vehicle alone (0.5% tragacanth);
(ii) d-d Nxtio at a constant volume of 24 ml/kg in the same vehicle;
(iii) d-l Nxtio at constant volume of 25 ml/kg in the same vehicle. The table 1 hereinafter reports the administration dosages.
              TABLE 1                                                     
______________________________________                                    
GROUP   TREATMENT VEHICLE DOSE mg/kg p.o.                                 
______________________________________                                    
1       vehicle           --                                              
2                         6.25                                            
3                         12.5                                            
4       d-d Nxtio         25.0                                            
5                         50.0                                            
6                         6.25                                            
7                         12.5                                            
8       d-l Nxtio         25.0                                            
9                         50.0                                            
______________________________________                                    
Forty five minutes later each rat received an injection of 0.1 ml of a 1% w/v suspension of carrageenan in sterile 0.9% saline, beneath the plantar aponeurosis of the left hind paw.
The volume of the paw was measured (in arbitrary units) before and 1.5, 3 and 6 hours after the irritant injection. The results are reported in the table 2, from which it can be observed not only that both diastereoisomers administered by oral route induce a significant inhibition of the carrageenan induced oedema, but also that d-l isomer is slightly less active than the d-d isomer.
                                  TABLE 2                                 
__________________________________________________________________________
Effects of oral administration of d-d Nxtio and d-l Nxtio                 
on a carrageenan-induced oedema in the rat                                
             DOSE                                                         
                 MEAN INCREASE       % INHIBITION                         
             mg/Kg                                                        
                 IN PAW VOLUME       OF SWELLING                          
GROUP                                                                     
     TREATMENT                                                            
             p.o.                                                         
                 1.5   3      6      1.5                                  
                                        3  6                              
__________________________________________________________________________
1    vehicle     7.9 ± 0.58                                            
                       12.1 ± 0.52                                     
                              13.4 ± 0.76                              
                                     -- -- --                             
2    d-d Nxtio                                                            
             6.25                                                         
                 3.7 ± 0.59                                            
                       5.5 ± 0.57                                      
                              8.1 ± 0.44                               
                                     53.2                                 
                                        54.5                              
                                           39.6                           
3            12.5                                                         
                 4.7 ± 0.95                                            
                       8.9 ± 0.90                                      
                              8.7 ± 1.12                               
                                     40.5                                 
                                        26.4                              
                                           35.1                           
4            25.0                                                         
                 4.3 ± 0.59                                            
                       8.3 ± 0.95                                      
                              9.8 ± 0.86                               
                                     45.6                                 
                                        31.4                              
                                           26.9                           
5            50.0                                                         
                 5.0 ± 0.94                                            
                       8.4 ± 0.76                                      
                              8.4 ± 0.86                               
                                     36.7                                 
                                        30.6                              
                                           37.3                           
6    d-l Nxtio                                                            
             6.25                                                         
                 4.1 ± 0.61                                            
                       6.2 ± 0.62                                      
                              8.7 ± 0.55                               
                                     48.1                                 
                                        48.7                              
                                           35.0                           
7            12.5                                                         
                 4.9 ± 0.92                                            
                       9.3 ± 1.10                                      
                              9.4 ± 1.12                               
                                     37.9                                 
                                        23.1                              
                                           29.8                           
8            25.0                                                         
                 4.6 ± 0.70                                            
                       8.9 ± 1.2                                       
                              10.2 ± 0.81                              
                                     41.7                                 
                                        26.4                              
                                           23.8                           
9            50.0                                                         
                 5.6 ± 0.92                                            
                       8.7 ± 0.8                                       
                              9.8 ± 0.84                               
                                     29.1                                 
                                        28.0                              
                                           26.8                           
__________________________________________________________________________
2. ran induced oedema in the rat
This test has been carried out like the preceding one, except that instead of carrageenan 0.1 ml of a 6% suspension w/v of dextran in the same sterile saline solution where injected.
The measurement of the paw volume (in milliliters) was carried out before the injection and at 0.5, 1 and 2.5 hours after the injection.
The results reported in the table 3 confirm the anti-inflammatory activity of both isomers, with a slight superiority of d-d isomer.
                                  TABLE 3                                 
__________________________________________________________________________
Effects of oral administration of d-d Nxtio and d-l Nxtio                 
on a dextran-induced oedema in the rat                                    
             DOSE                                                         
                 MEAN INCREASE     % INHIBITION                           
             mg/Kg                                                        
                 IN PAW VOLUME     OF SWELLING                            
GROUP                                                                     
     TREATMENT                                                            
             p.o.                                                         
                 0.5   1     2.5   0.5                                    
                                      1  2.5                              
__________________________________________________________________________
1    vehicle     1.09 ± 0.05                                           
                       1.28 ± 0.04                                     
                             1.08 ± 0.06                               
                                   -- -- --                               
2    d-d Nxtio                                                            
             6.25                                                         
                 1.03 ± 0.04                                           
                       1.00 ± 0.03                                     
                             0.72 ± 0.04                               
                                   5.5                                    
                                      21.9                                
                                         33.3                             
3            12.5                                                         
                 1.12 ± 0.06                                           
                       1.16 ± 0.04                                     
                             0.83 ± 0.06                               
                                   0   9.4                                
                                         23.2                             
4            25.0                                                         
                 1.09 ± 0.02                                           
                       1.11 ± 0.04                                     
                             0.81 ± 0.03                               
                                   0  13.3                                
                                         25.0                             
5            50.0                                                         
                 1.24 ± 0.05                                           
                       0.90 ± 0.04                                     
                             0.73 ± 0.02                               
                                   0  29.7                                
                                         32.4                             
6    d-l Nxtio                                                            
             6.25                                                         
                 1.04 ± 0.08                                           
                       1.03 ± 0.07                                     
                             0.85 ± 0.07                               
                                   4.6                                    
                                      19.5                                
                                         21.3                             
7            12.5                                                         
                 1.11 ± 0.04                                           
                       1.11 ± 0.08                                     
                             0.79 ± 0.08                               
                                   0  13.3                                
                                         26.8                             
8            25.0                                                         
                 1.12 ± 0.06                                           
                       1.14 ± 0.06                                     
                             0.80 ± 0.06                               
                                   0  11.0                                
                                         26.0                             
9            50.0                                                         
                 1.20 ± 0.05                                           
                       1.10 ± 0.04                                     
                              0.9 ± 0.04                               
                                   0  14.0                                
                                         16.6                             
__________________________________________________________________________
3. Writhing test in the rat
Groups of 10 rats (Wistar-Charles River) were dosed orally with either vehicle (0.5% tragacanth) or test compounds (d-d and d-1 Nxtio) at a costant volume of 10 ml/kg according to the treatment table 1.
Forty-five minutes later each rat received an intraperitoneal injection of 1.0 ml of 1% solution of acetic acid. They were then placed in individual cages and the number of writhes elicited by each rat in the following 25 minute period was recorded.
The results of this test are reported in the table 4, from which it can be observed that both diastereoisomers cause a dose dependent inhibition, with a marked superiority of the isomer d-d of the order of 20%.
                                  TABLE 4                                 
__________________________________________________________________________
Analgesic activities of orally administered compounds in                  
the writhing test - individual animal data                                
                NUMBER OF           MEAN                                  
        ORAL DOSE                                                         
                WRITHES/25 MIN FOR ANIMAL No.                             
                                    WRITHING SCORE                        
TREATMENT                                                                 
        (mg/Kg) 1 2 3 4 5 6 7 8 9 10                                      
                                    (± s.e.)                           
__________________________________________________________________________
Vehicle --      49                                                        
                  54                                                      
                    40                                                    
                      65                                                  
                        43                                                
                          48                                              
                            23                                            
                              65                                          
                                19                                        
                                  57                                      
                                    46.3 ± 5.24                        
d-d Nxtio                                                                 
        50       4                                                        
                  10                                                      
                    16                                                    
                       4                                                  
                        24                                                
                           4                                              
                             8                                            
                               6                                          
                                 3                                        
                                   1                                      
                                     8.0 ± 2.36                        
        25      35                                                        
                   7                                                      
                    16                                                    
                      16                                                  
                         5                                                
                          36                                              
                            16                                            
                              36                                          
                                23                                        
                                  21                                      
                                    21.1 ± 3.81                        
        12.5    42                                                        
                  61                                                      
                    23                                                    
                      25                                                  
                        39                                                
                          48                                              
                            38                                            
                              43                                          
                                 9                                        
                                   7                                      
                                    33.5 ± 5.74                        
        6.25    47                                                        
                  59                                                      
                    33                                                    
                      46                                                  
                        71                                                
                          23                                              
                            26                                            
                              25                                          
                                24                                        
                                  47                                      
                                    40.1 ± 5.52                        
d-l Nxtio                                                                 
        50       7                                                        
                  12                                                      
                    10                                                    
                       8                                                  
                        24                                                
                           7                                              
                            11                                            
                               5                                          
                                 9                                        
                                   0                                      
                                     9.3 ± 1.95                        
        25      24                                                        
                  15                                                      
                    32                                                    
                      15                                                  
                         7                                                
                          28                                              
                            25                                            
                              31                                          
                                20                                        
                                  25                                      
                                    22.2 ± 2.51                        
        12.5    56                                                        
                  65                                                      
                    31                                                    
                      37                                                  
                        44                                                
                          52                                              
                            35                                            
                              41                                          
                                25                                        
                                  10                                      
                                    39.6 ± 5.03                        
        6.25    48                                                        
                  51                                                      
                    45                                                    
                      39                                                  
                        31                                                
                          34                                              
                            46                                            
                              37                                          
                                26                                        
                                  72                                      
                                    42.9 ± 4.09                        
__________________________________________________________________________
4. Randall-Selitto test in the rat
Male Wistar rats (70-90 g) were starved 18 hours prior to the commencement of the experiment but water was available ad libitum.
Each rat received an injection of 0.1 ml of a 20% suspension of Brewer's yeast in distilled water beneath the plantar aponeurosis of the left hind paw.
One hour later the pain thresholds of both the inflamed (yeast injected) and normal hind paw were measured using an analgesiometer designed by U. Basile; the animals were then dosed orally with vehicle (0.5% tragacanth) or test compounds at a constant dose volume of 10 ml/kg.
There were 10 rats in each drug-treated group and 20 rats in the vehicle-treated group.
The pain thresholds of the inflamed and normal hind paws were again measured at 1, 2 and 4 hours after dosing.
The results are reported in the table 5 from which it can be observed not only a peak of analgesic effect at two hours from the administration but also the superiority of the (d-d) isomer.
                                  TABLE 5                                 
__________________________________________________________________________
Changes in pain threshold of inflamed and normal paws of rats             
receiving oral treatment with d-d Nxtio and d-l Nxtio                     
                 MEAN CHANGE IN PAIN THRESHOLD (G ± S.E.)              
                 FROM PRE-DOSE AT POST-DOSE TIME                          
           DOSE  1 HOUR         2 HOURS        4 HOURS                    
      TREAT-                                                              
           (mg/Kg)                                                        
                 INFLAMED                                                 
                         NORMAL INFLAMED                                  
                                        NORMAL INFLAMED                   
                                                       NORMAL             
GROUP MENT p.o.  PAW     PAW    PAW     PAW    PAW     PAW                
__________________________________________________________________________
1     vehicle                                                             
           --    -22.4 ± 15.2                                          
                         -40.5 ± 17.8                                  
                                -42.0 ± 15.1                           
                                        -52.6 ± 18.0                   
                                               -21.3 ± 15.3            
                                                       -39.2 ± 13.9    
2     d-d Nxtio                                                           
           6.25  -27.2 ± 30.8                                          
                         -12.8 ± 17.8                                  
                                -42.2 ± 21.9                           
                                        -17.7 ± 18.2                   
                                               -32.7 ± 15.5            
                                                       34.1 ± 17.4     
3          12.5  32.6 ± 40.1                                           
                         -13.7 ± 22.9                                  
                                32.6 ± 41.7                            
                                        -23.4 ± 18.2                   
                                               38.9 ± 48.6             
                                                       10.7 ± 23.7     
4          25    53.2 ± 29.9                                           
                          -1.0 ± 26.0                                  
                                31.3 ± 35.8                            
                                        -33.5 ± 24.4                   
                                               41.9 ± 35.3             
                                                       18.7 ± 35.9     
5          50    48.3 ± 27.9                                           
                          -1.3 ± 22.9                                  
                                98.9 ± 38.9                            
                                        -38.8 ± 18.9                   
                                               79.4 ± 42.7             
                                                       25.7 ± 24.3     
6     d-l Nxtio                                                           
           6.25  -21.6 ± 30.9                                          
                         -14.3 ± 20.0                                  
                                -38.4 ± 18.9                           
                                        -24.5 ± 25.3                   
                                               -23.1 ± 18.4            
                                                       -10 ± 25.5      
7          12.5  25.5 ± 37.3                                           
                         -15.4 ± 29.6                                  
                                20.5 ± 38.7                            
                                        -20.9 ± 25.6                   
                                               21.2 ± 43.2             
                                                       -12 ± 15.8      
8          25    40.2 ± 31.4                                           
                         -10.8 ± 27.5                                  
                                23.2 ± 34.6                            
                                        -31.5 ± 21.9                   
                                               29.6 ± 38.1             
                                                         19 ± 37.7     
9          50    42.3 ± 31.6                                           
                          -1.4 ± 10.3                                  
                                60.2 ± 45.7                            
                                        -38.4 ± 22.8                   
                                               52.1 ± 19.1             
                                                         18               
__________________________________________________________________________
                                                       ± 22.7          
At this point it is worth to noting that the advantages achieved by the present invention must be evaluated as a function of the relevant advancement already achieved with the compounds of the European Patent 124.925 whereby the further improvement which is thus obtained is, in obviously relative terms, a result relevant as well and fully unforeseable.
The pharmaceutical compositions according to the present invention comprise as the active ingredient the (d-d) diastereoisomer together with the standard vehicles and excipients.
In this connection reference is made to the disclosure of European Patent 124.925, which is here incorporated for reference.
The dosages of active principles shall be still those of the corresponding composition based on Naproxen whereby the therapeutical effect is obviously increased.

Claims (2)

We claim:
1. A method for achieving anti-inflammatory and analgesic effect in a patient in need of such treatment which comprises administering to such patient an effective amount of S-d-2-mercaptopropionamido acetic acid.
2. A pharmaceutical composition useful in achieving anti-inflammatory and analgesic effect in a patient and suitable for administration by oral, topical or rectal route which comprises an effective amount of S-d-2-mercaptopropionamido acetic acid and a pharmaceutically acceptable carrier therefor.
US07/485,084 1990-01-29 1990-02-26 D-2-(6-methoxy-2-naphthyl)-propionic acid and pharmaceutical compositions containing it Expired - Fee Related US5093361A (en)

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IT19184A IT1238679B (en) 1990-01-29 1990-01-29 OPTICALLY ACTIVE DERIVATIVE OF D-2- (6-METHOXY-2-NAFTIL) ACID - PROPIONIC AND PHARMACEUTICAL COMPOSITIONS CONTAINING IT
IT19184A/90 1990-01-29

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Cited By (1)

* Cited by examiner, † Cited by third party
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US5223516A (en) * 1990-03-22 1993-06-29 E. R. Squibb & Sons, Inc. 3,3,3-trifluoro-2-mercaptomethyl-N-tetrazolyl substituted propanamides and method of using same

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EP0440098B1 (en) 1995-04-05
ATE120731T1 (en) 1995-04-15
EP0440098A1 (en) 1991-08-07
KR970011456B1 (en) 1997-07-11
DE69108580D1 (en) 1995-05-11
IT9019184A1 (en) 1991-07-30
ES2071843T3 (en) 1995-07-01
IT1238679B (en) 1993-09-01
IT9019184A0 (en) 1990-01-29
DE69108580T2 (en) 1996-11-28

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